5.1 μm Ion-Regulated Rigid Quasi-Solid Electrolyte Constructed by Bridging Fast Li-Ion Transfer Channels for Lithium Metal Batteries.

An ultra-thin quasi-solid electrolyte (QSE) with dendrite-inhibiting properties is a requirement for achieving high energy density quasi-solid lithium metal batteries (LMBs). Here, a 5.1 μm rigid QSE layer is directly designed on the cathode, in which Kevlar (poly(p-phenylene terephthalate)) nanofibres (KANFs) with negatively charged groups bridging metal-organic framework (MOF) particles are served as a rigid skeleton and non-flammable deep eutectic solvent (DES) is selected to be encapsulated into the MOF channels, combined with in-situ polymerization to complete safe electrolyte system with high rigidness and stability. The constructed topology network demonstrates high rigidity (5.4 GPa), high ionic conductivity (0.73 mS cm-1 at room temperature), good ion-regulated properties, and improved structural stability, contributing to homogenized Li-ion flux, excellent dendrite suppression and prolong cyclic performance for LMB. Additionally, ion regulation influenced the Li deposition behavior, exhibiting a uniform morphology on the Li-metal surface after cycling. According to density-functional theory (DFT), KANFs bridging MOFs as hosts play a vital function in the free-state and fast diffusion dynamics of Li-ions. This work provides an effective strategy for constructing ultrathin robust electrolytes with a novel ionic conduction mode. This article is protected by copyright. All rights reserved.